Method of treating organic material and apparatus therefor



June 29 9 @926 E. TAYLQR METHOD OF TREATING ORGANIC MATERIAL AND APPARATUS 'IIIEREF'OFI- Filed June 2l, 1924 INVENTOR 5% I l i www mw m, n W

av I

ATTORNEY treatment or use.

Patented June 29, 1926.-

i y 1,59aan es rA'rENfTjo-FFi-ce.-

nnwm "rAYLoR, 0F BnooxLYmNnw vomi,- AssIcNoR-To TAYLOR LABonA'ronms,V

INC., OF NEW YORK, N. Y., A CORPORATION OF NEW YORK.

` Marston or :rneA'riNe ORGANIC MATERIAL AND APPARATUS rnnnnson.

Application nea :une 21,1924. serial Harmsen.

-My invention relates to improvements in methods 'of treating organic material and apparatus therefor. The main .object of the invention is to provide improvements whereby certain kinds of organicand other material may be conveniently and efficiently put into solution and the solvent constituents .then removed therefrom, leaving the material in'- orm -convenient; for further Further and more specitie objects, features and advantages-will more clearly appear from the detail description given below taken in connection with the accompanying sheet ot drawings `Awhich form a part of this specification.

In`the drawings, Fig. l is a vertical section,' largel v diagrammatic, illustrating an apparatus embodying the main features of my invention in oneA form. Fig. 2 is a similar view illustrating the electrolytic cell of Fig. 1 with additional electrodes thereinl Fig. 1) is a vertical section illustrating one forni of apparatus suitable for treating certain organic materials from the apparatus of I1" igs. 1 and 2 'or certain purposes.

While my improvements may he usefully applied to various organic materials as wel-l as other materials, I have found it particularlvuseful in connection with the treatment of cellulosic material and will, therefore, deseribe'the invention in connection with the treatment of cellulosic material for the production ot cellulose products.

Referring to Fig. 1. 4 represents a tank or chamber substantially lilled with, in the present instance, the solvent solution of cellulose 5 such as a solution or cupro-ammonia in water. Other solutions, however, upon the material metatl ammonia;ll solutions may be used such as nickel ammonia solution. The chamher tis provided with a supporting screen .6 near-its bot-toni adapted to permit the solution to pass therethrough and on this screen is placed the cellulosic or other material 7 tay-be* dissolved. Leading from the top of the chamber 5 is a pipe 8 adapted to confvcy- .the Asolution from .the chamber 5 dish i shaped memherrlQ-,the -lower face :of-which vis covered .undissolved pieces of'cellulosic material frornbeingcar-Q through the inverted) tively.

with a valve at y11` and extends to a worm 12 in a chamber 13 `filled with cooling Water 14, the water being introduced at the bot-.v tom through pipe 15 and,overtlowing at A the top. through pipe` 16j. 17r represents a pipe connected with arsupply ot' ammonia gas under pressure or liquidammonia, which is 111]' ected. into the solution passing through the pipe. 8 by means of a valved injector 18. l

rom the cooling. lorm 12 the vsolution passes through pipe 19 and through valve 2O tomanifold pipe 21.; 22 represents an ',-electrolytic cell 4provided in the present in.

stance' with a series of copper electrodes 23,

alternate electrodesct23.' beingelectrically,E

connected with bus ,bars 24and V25 respec. The cell .22.;is, sealed with, a cover 2G and carries4 a pressure gage 27 forindieating the pressure within the cell. The cover is also provided with an exhaust 'pipe 28 having a. valve at`29 through which am# monia. and other gases may be` withdrawn 21 passes into the spaces in 'the cell 22 between the electrodes 23 through valve connections 30. Thefsoluti'pnis withdrawn from the top of the cell' bymeans of the pipe 31through connections 32. The solu-4 tion is withdrawn through pip'e 31 by' means of a pump 33 and forced to return to the chamber 4 through pipe 34 provided with.- a valve :1t- 35; yThe chamber 4 is sealed with a cover 36 'also Erovided with a pressure gage 37 for in icating the pressure withinthe chamberf4 and the cover. 36 is. provided with an aperture through which the cellulosic or other material to be dissolved maybe inserted, which aperture is normally sealed by cover 38. The inverted vwhen desi-red.` The solution in the manifold dish r shaped member 9 is also .connected l l 55. a direct current is caused to ass between the circulated through the tank13. The pump 33 is started to circulate the water withdrawing same from chamber' 4 through-pipe 8, cooling coil 12 to pipes 19 and 21 and into '5 the cell 22, whence it 1s withdrawn through pipe 31, pump 33 andforced through pipe 34 back through the chamber 5. The ammonia 'gas under pressure is 'introduced through the nozzle 18 and soon the water 10 becomes more or less saturated with .am-

monia as it travels in its cyclic path back and forth between the chamber 4 and the cell 22. The bus bars 24 and 25 are connected. to a source of alternating current thereby l l5 causing an alternating current tapass between the alternately arranged copper electrodes 23.' This causes the copper from these copper electrodes to be kicked oli therefrom electrolyticallyA and dissolved in the am- 2Q monia'so'lution thereby forming a cupro-ammonia st\lution. The celluloslc material 7 v tobe dissolved-having been inserted in the chamber 5,and the .cupro-ammonia solution being thus` circulated therethrough will 2`r4gradually dissolve morel andv more of the cellulosic material' and the solution travelling in'this cyclicpath and through the electrolytic cell 22, will gradually have its strength of cupro-ammonia built up by the continual I ,'30 electrolytic removal of copper IOIII the elc" trodes 23,. which passes into the solution. The ammonia content ofthe solution may be built upvas desired by regulating the valved `nozzle 18. The cyclic operation is'continued 35 until the strength of the solution in cellulose has been built up to the desired point, or

until this. solution contains as much dissolved cellulose as is possible and still leave it notA too thick for lconvenient handling.'

Thenpump 33`is stopped and the valvesll, 18, 45 and 20 are'closed and lthe cover 26 removed and an additional set of'electrodes4 inserted as shown in Fig'. 2. These additional electrodes are indicated in Fig. 2 at 46. They are inserted between the electrodes 23 and are electrolytically connected to abus bar 47. `The electrodes 46 may be made of antimony-lead (Say .40% lead and 60% antimong and 'after inserting these electrodes t e cover 26 is replaced and bothof. the bars 24V and 25 are connected to the negative terminal of. a source of direct cur'- rent while the bar'47 is "connected'tov-thc I' positive 'terminal or -pole thereof. Thereby A be 'acted upon electrolytically whereby cel- I .6 lolo/se is osited upon the' anodes 46 in` electrodes ,46 as anodes an the -'electrodes 23 as cathodes. 'This causes the' cupro-am- Axn'onia solution of cellulose in the cell 22 to laygrsasin icated at 48 while the copper of 'the -sol'veht is caused to deposit electrol -v from impurities such as any dyes, etc. in the little value;

the making of smokeless powder,

more or less of the copper tlereav fromin the first-operation', and the ammonia is freed and such of it as is volatilized may be `collected through pipe 28 and condensed forreQuse. After substantially all the solvent constituents have been removed rom 7G the dissolved cellulose in the cell'22 and the cellulose has been substantially all deposited o n `the anodes 46, the cover 26 is removed and the anodes 46 removed andthe cellulose stripped therefrom for further treatment 75 l' and use.

While this operation of removing the sol` vent constituents electrolytically from the dissolved cellulose Ahas been going on, the chamber 4 may be connected by means of '8 pipes 41 and 39 to another cell and' cooler like the cell 22 and cooler 13 for the purpose of building up another cell full of dissolved cellulosic material. lVhen this is done the electrodes 46 afterA the cellulose has been stripped therefrom or other electrodes, 46 may be inserted in the second cell in the same manner as above described and the cel; lulose deposited thereon and the solvent con-l sti-tuents removed inlike manner and while this is going on a fresh batch of cellulose solution may be. built up'in the-original cell 22 thereby forming an apparatus 'and arrangement whereby cellulose material is being substantially continuously dissolved and the solvent constituents removed therefrom and the cellulose deposited electro.- lytically. During these cyclic operations the electrodes 23 may suflier some additive loss of copper which however, may. be replaced by adding finely divided copper to the tank 4 as occasion may require. l

The condition ofthe cellulose deposited will depend lnoxeor less on the current denlo l sity. If a low current density is used the I cellulose will be vdeposited ina relativelyf tough iiexible film.` IfLhowevelt, a high cur-`v rent density is used. the 'cellulose will be de* posited thereon in a more or less porous,y spongyor soft condition. I have found that h .1 byusing a voltage of four volts and an axn f perage of 200 amperes in a cellemploying Y 10 anode plates,.each 16 inches -by 10 inches,

that a medium ldeposit is produced.T The cel.- ni I luloseisdeposited in a more or less white or transparent condition substantially free orinal cellulosic material introducedin'th'e ta 4, these impurities beingleft in thes' luton.. This is advantageous since it permits Vof thev use as raw materialof old ra and fabrics and various kinds, otherwise avia@ es 46 may be treated inany suitable wai for p oto- 1 graphic, films, imitation lleather and other; u ses including the various ways mentioned in"y i prior. applications Ser, No. 341,953, filed Dec.- 2', 1919, Ser. o. 364,960, filed Mar. 11, 1920.

The cellulose recovered from the elec en. v

,` If5 the lcellulose Jis deposited in a somewhat softi'or spongy-conditiom it may b'e stripped -from theelectrodes 46 and then-broken up or "relativelylinely divided by pressing `the- A' iiiz'iterialA may then be 'washed byipouring waterinto the cylinder 50 until it completely In this Way the material may lie-washed in running water to remove any zimmonialeft in the niaterizil.- rllien While the material is siibstantially surrounded with water, acetone :oijalcohol may be poured into the cylinder on top'ot' .the water and cellulose material,

.the acetone and alcohol being lighter than 'the'vvateewill remain on top, but will 'gradually djcend' as the water is permitted toi; dehydrate the inelydivided cellulose -matefnf rialn'nd after the water isthus removed the be driven 'oil'.

, or 'making cclluloid1 etc. or for making fresh i regulated so that. the `water fpasses out slowly and. theacetone or alcoholfollows, down slowly and stilistantially completely'replacesI the water. ,711s alcoli l andacetone act toveiiy completelyfj These organic compounds such addition ol' dehydrating agent'is stopped'and thc deliydrating agent reniovedthrough the valve 52 as far as maybe-andthe cellulose issealed (except for a pipe to fcarry away thc 'vo'atilized acetone or the like) thereby causing the remaining dehydrating agent to This leaves thecelluIOse in;

the'form ot' a dry' fine powder, `suitable for lacepoiviiler, surgical dressing powder, for l I terial whichconsists in dissolving cellnlosic` nilrating, for filling for smokeless powder,

l' and scope of the improvements in-thein modifications and forms coming within th Whic l have described my improvements.

changes or modifications 4may be made and the invent-ion embodied 18e, widely dili'erent' forms without departing-rrom the spirit 'broader aspects; hence I desire to Coverall language or scope of any oneor more of the appended claims.

' v'What I claim as new and-desire -to secure b v Letters Patent is:

1. The method oftreatingorganicI material which 'consists in 'dissolving'organi@ material in ajsolvent'solutipn thereof Ain enel said?solutionP to v :'m'ot-lier-'f- 1 chamber; increasing-'thestrengtlr offlt-he Qsol-'ff l -iaeausingfelieisoluton to dissolve more A991111# vent solution V'in the secondichambergfre'tnrn-- in the solution to the first chamber tadisso ve more organic material therein,

-same through ascreeii and tlien placing inI a cylinder 5,() as'shown in Fig. 3 provided with "a's'creenl at 'the 'bottom theieof for sup-- i "poi'ting' the material in the cylinder. The

and

continuing the cyclic-'1,transfer-of the solution until the desired amount ot organic -material has been dissolved therein.v

2. Thel method oftreating organic matc- -rial-whichconsists iii-dissolving organicmaterial in 'a metal -compoundsolvent solution building up of the'solution until the desired amount .of `organicmaterial has beenv dissolved therein. i

g3. The method off treating organic material which consistsin l dissolving organicl material in'a metalj'compound solveii'tfsolu tion thereof inA a -fchan'iber, removing the 'solution from? saidhainben increasinr the `strengtliot the"solventgsolution by -a ding metal theretolelectrolytically, returning the strengthenedsdlution to the said chamber toi'vdissolv'' more organic ,material Athe-rein. and continuing: 'said cyclic;v transfer and building 4up o'f the sA lution until the desired solved therein, andthen removing solvent constituents Ifrom :the dissolved organic 4ma terial. byV electrolytieaction.

4. The method` of `treating cellulosic ina- .terial which consists in dissolving cellulosic iii-1y be then dumped into a ball mill ivhicl material in a@ metal ammoniasolvent there of in=a chamber, removing the solution from the chamber,and adding more of the metal thereto by"electrolytic action, and returning yccllulo'sic tmaterial.

5. The method oftreating cellulosic mamaterial in ametalammonia solvent therei of, .building up the solution by adding more of-'the metal thereto by .electrolytic action and causing A:the solution todissolve more cellulosic material.

Thef'metliodfof-treating -celliilosic material whichconsists-in dissolving cellulosic material in. a.metal-antimonia 'solvent thereof, building up the solution by adding more 'and 'causing' thesoIution 'to dissolve more e(.cellulosic material, '.-and finally removing 4solvent constituentsfrorn the dissolvedcellu losic material by electrolytic action;

7. The method ofdissolving cellulosic material which consistsin dissolving somecel` lulosic material in a metalammoniaso1vent thereof, subjectingthe; solution,l to electro. lyticV actiomofan alternating current between added to?v thsSQlilliQlf1168trolyticallyIlv :and

' losie material.

8.A The method which consists in subjectthereof'in a `chamber,'removing the solution from said chambei',increasing the strength velectrodes?"of the. metal, ,wlierebyametal is aniount o'f organicimiterial .has Abeen dis.

the solutionto the chamber to dissolve more of the metaltheretorby 4electrolytie action l ing a' metal-ammonia solutioiito. electrolytic action of an alternating' current between electrodes of the metal whereby Ametulfrom rial therein while the solution is circulating.

the electrodesv is added to the solution.

9. The method which consists in object-- ing a metal-ammonia solutionto electrolytic actlon of an alternating current between and passing a. current between-electrodes of the cell durin the circulation 'to increase the strength o the solution.

12.1The method which consists in circulatl ing a metal-anim nia solution through an electrolytic cell, s'solving cellulo'sicmate- 'rial therein'while the solutionis circulating 'and passing`an alternating current between electrodes-of the metal'in the cell during the circulation to increase the strength of the solution and' dissolve more cellulosic material therein. I l

13. The .method which consists in circulatin'g a vmetal-ammonia solution through .an

electrolytic. cell, dissolvin cellulosic material in the'solutio'n whilst e solution is circulating and passing an alternatingcurrent between electrodes ofthe metal in the cell during the vcirculation -to increase the strength of .the solution` and-#dissolve more cellulosic material in the solutinnnecting said electrodes to the negntv pole of a source of direct current, causing said electrodes to act as cathodes, inserti` rating anodes in the cell betweenl said cat odes increase thestxn h'o adding ammonia and subjecti the solution to direct current electrolysis to remove solvent constitu ents from thesolution of oellulosic material and deposit cellulose on the anodes..

14.1The method l'which consistsffin circulating sfmetal-axnmonia solution through an clectrolytic cell, dissol'vn celluloslc mate- 4rial in the `solution while t e solution is circulatingnnd ps trodes ofthe cell uri =thefcirculation o the solution, and

circhlation.

4 15. Ehe method which consists 1n circu- 'lating a me|ta1-ammonia solution through an -.electrolyti,e,' cell, dissolving cellulosic material in theselution while the solution is circulating and passing a current between elec- 'action and dissolving' ancurrent betweenvelef.

the solution during the trodes 'of the cell during the circulation to increase thestrength ofthe solution, and adding ammonia tothe solution during the circulation, and cooling the solutionn during the circulation.

16. The method which consists in circulating n metal-.ammonia solution through an electrolytic cell, dissolving cellulosic material in the solution Whilethe solution iscirculatingr and passing an alternating current between electrodes of the metal in the cell dur- .ing the circulationto increase the strength of the solution and dissolve more cellulosic materal in the solution, adding ammonia to the solution and cooling the solution during the circulation.

17. The method which consists in circulating a metal-ammonia. solution through an electrolytic cell, dissolving cellulosic material in the solution While the solution 'is circulating and passing an alternating current between electrodes ofthe metal in the' cell during the circulation to increase the strength of the solution 'and dissolve' more cellulosic material in the 'solution,'and then passing a 'direc-t current between electrodes in the solution in the cell to remove solvent.

constituents from the dissolved cellulose undl 'deposit cellulose.

18. The method'of treating cellulo'sic'ma tcrial whichv consists in forming s; solution.

thereof in av Imetal-ammo'nia solution, subjecting `the solution .to electrovltic action to remove solvent constituents from the dissolved cellulose, displaci Athe water from the-resultant cellulosewith a. volatile oranic dehydrating agent, and volatilizin'g t e dehydrating agent from the cellulose.

19. `The method which consists in dissolvinncellulosic material in a metal-ammonia solvent thereof, subjecting the' solution to electrolytic action to remove solvent constituents from the dissolved cellulosethe electrolytic current density being such as to deposit the'cellulose in spongy soft condition,

removing the cellulose and breaking it up and displacing the water from the resultant cellulose with a volatile organic dehydrating agent, and volatilizing the dehydrating agentfrom the cellulose.; y

20. The method which consists in dissolving cellulosic ms.terial, removing solvent constituents therefrom, breaking up there- ,sultant cellulose and displacing the water 'from the1 rlesiltant cellulose wth alvolatile organic e y rating agentv an vo atihzih' "the dehydrating agent from the cellulo g 21.- In an apparatus of the. clam descri d the combination of an" electrolytic cell, a.

chamber for dissolving organic material..

for transferring the .solutherein, meab tion of orga c' material from the chamber to the ce said having metal electrodes energized by4 alternating current wherebyan alternating current is 'caused to 130 pass between the electrodes and cause metal therefrom to enter the solution in the Cell, and means for conveying the solution back to the container to'dissolve more organic material.

2:2. In an apparatus of the class described .the combination of an eiectrolytio cell. a

chamber for dissolving organic material therein, means for transferring the solution of organic material from the chamber to the cell, said cell having metal electrodes energized by alternating' @'rrent whereby an alternating current is Caused to pass between the electrodes and cause metal -therefroin to enter the solution in the cell,

chamber for dissolving organic material;

therein, means for transferring the solution of organic material from the chamber to the cell, said cell having metal electrodes energized by alternating current whereby an alternating current is caused to pass between the electrodes and cause metal therefrom to enter the solution in thel cell, means for conveying the solution back to the container to dissolve more organic materiel, means for cooling,r the solution on its Way between the Chamber and the Celli, and means for addingreagent to the solution on its Way between the chamber and the cell.

24. in an apparatus of the class described the combination of an electrolytie oeil, a chamber for dissolving organic material therein, ineens for transferng the solution s of organic niateriai from tile chamber to the Cell, said cell having metal electrodes energized by alternating current whereby an alternating currentis Caused to pass hetween the' electrodes and cause rnetai therefrom to enter the solution in the ee i, means for 'conveying the solution haeltF to the Qontainer to dissolve more erganie material, and electrodes adapted to be inserted between said first inentioMfl eleetrodes in the cell andupon passing a t current bef tween said first mentioned electrodes end said last mentioned electrodes', to have inaterial from said sointion electro-deposited l thereon. 

